Ground-based Multi-Axis Differential Optical Absorption Spectroscopy (Max-DOAS) measurements of nitrogen dioxide (NO₂) were continuously obtained from January to November 2019 in northeastern China (NEC). Seasonal variations in the mean NO₂ vertical column densities (VCDs) were apparent, with a maximum of 2.9 × 10¹⁶ molecules cm⁻² in the winter due to enhanced NO₂ emissions from coal-fired winter heating, a longer photochemical lifetime and atmospheric transport. Daily maximum and minimum NO₂ VCDs were observed, independent of the season, at around 11:00 and 13:00 local time, respectively, and the most obvious increases and decreases occurred in the winter and autumn, respectively. The mean diurnal NO₂ VCDs at 11:00 increased to at 08:00 by 1.6, 5.8, and 6.7 × 10¹⁵ molecules cm⁻² in the summer, autumn and winter, respectively, due to increased NO₂ emissions, and then decreased by 2.8, 4.2, and 5.1 × 10¹⁵ molecules cm⁻² at 13:00 in the spring, summer, and autumn, respectively. This was due to strong solar radiation and increased planetary boundary layer height. There was no obvious weekend effect, and the NO₂ VCDs only decreased by about 10% on the weekends. We evaluated the contributions of emissions and transport in the different seasons to the NO₂ VCDs using a generalized additive model, where the contributions of local emissions to the total in the spring, summer, autumn, and winter were 89 ± 12%, 92 ± 11%, 86 ± 12%, and 72 ± 16%, respectively. The contribution of regional transport reached 26% in the winter, and this high contribution value was mainly correlated with the northeast wind, which was due to the transport channel of air pollutants along the Changbai Mountains in NEC. The NO₂/SO₂ ratio was used to identify NO₂ from industrial sources and vehicle exhaust. The contribution of industrial NO₂ VCD sources was >66.3 ± 16% in Shenyang due to the large amount of coal combustion from heavy industrial activity, which emitted large amounts of NO₂. Our results suggest that air quality management in Shenyang should consider reductions in local NO₂ emissions from industrial sources along with regional cooperative control.

The most prominent source of Cu contamination in soils is metal mining and processing, partly since the Middle Age. However, coal mining and combustion can also cause (some) Cu contamination. We studied the distribution of Cu concentrations and isotope ratios in soils of the Huaibei coal mining area. The contribution of the coal mining and combustion to total Cu concentrations in soil was determined with a two-end-member mixing model based on the distinct δ⁶⁵Cu values of the Cu emitted from coal mining and combustion and in native soil. The mean Cu concentration of 75 mg kg⁻¹ exceeded the local soil background value (round to 22.13 mg kg⁻¹). The similar δ⁶⁵Cu value of grass near the coal mining and combustion operation as in gangue and flying ash indicated a superficial Cu contamination. Mining input was the dominant source of Cu in the contaminated soils, contributing up to 95% and on average 72% of the total Cu in the topsoils. The mining-derived Cu was leached to a depth of 65 cm, where still 29% of the Cu could be attributed to the mining emissions. Grasses showed lower δ⁶⁵Cu values than the topsoils, because of the preferential uptake of light Cu isotopes. However, the Δ⁶⁵Cugᵣₐₛₛ₋ₛₒᵢₗ was lower in the contaminated than the uncontaminated area because of superficial adsorption of isotopically heavy Cu from the mining emissions. Overall, in this study the distinct δ⁶⁵Cu values of the mining-derived Cu emissions and the native soil allowed for the quantification of the mining-derived Cu and had already reached the subsoil and contaminated the grass by superficial adsorption in only 60 years of mining operation.

Soil polycyclic aromatic hydrocarbons (PAHs) generated from industrial processes are highly spatially heterologous, with limited quantitative studies on their main influencing factors. The present study evaluated the soil PAHs in three types of industrial parks (a petrochemical industrial park, a brominated flame retardant manufacturing park, and an e-waste dismantling park) and their surroundings. The total concentrations of 16 PAHs in the parks were 340–2.43 × 10³, 26.2–2.63 × 10³, and 394–2.01 × 10⁴ ng/g, which were significantly higher than those in the surrounding areas by 1–2 orders of magnitude, respectively. The highest soil PAH contamination was observed in the e-waste dismantling park. Nap can be considered as characteristic pollutant in the petrochemical industrial park, while Phe in the flame retardant manufacturing park and e-waste dismantling park. Low molecular weight PAHs (2–3 rings) predominated in the petrochemical industrial park (73.0%) and the surrounding area of brominated flame retardant manufacturing park (80.3%). However, high molecular weight PAHs (4–6 rings) were enriched in the other sampling sites, indicating distinct sources and determinants of soil PAHs. Source apportionment results suggested that PAHs in the parks were mainly derived from the leakage of petroleum products in the petroleum manufacturing process and pyrolysis or combustion of fossil fuels. Contrarily, the PAHs in the surrounding areas could have been derived from the historical coal combustion and traffic emissions. Source emissions, wind direction, and local topography influenced the PAH spatial distributions.

Residential coal combustion is a prominent source of brown carbon (BrC) aerosols, but knowledge of their molecular structures and optical absorption were limited, which have notable used in ambient BrC source identification and radiative forcing calculation. In this study, the Fourier transform–ion cyclotron resonance mass spectrometry combined with partial least squares regression analysis as well as Fourier transform infrared spectroscopy analysis were used to insight the molecular compounds and structures of BrC from anthracite and bituminous coal combustions between traditional and improved stoves. The absorption Ångström exponents (AAE) and mass absorption efficiency (MAE) values for the BrC emitted from the combinations of bituminous were both 1.2–2.5 times lower than those of anthracite, interpreting that the BrC from the anthracite emissions had greater light-absorbing capacity. In contrast, the emission factor of light absorption (EFAbₛ) at 365 nm for the bituminous coal combusted in the traditional stove was the highest among all the tested scenarios, which revealed that the incomplete combustion of bituminous coal could emit more BrC. It was noted that primary BrC emitted from the coal combustion with traditional stoves contains higher aromaticity groups of C–C and C＝O and higher S containing organics, whereas more aliphatic groups were found in BrC using the improved stoves. N-containing (CHON and CHONS) compounds were dominated in the total molecular formula of BrC, whereas the sum of CHON and CHO groups had high double-bond equivalent (DBE) values contributed 53.5%–87.1% to the total BrC absorption. Moreover, for CHOS, the lowest of estimated molecular absorption, DBE, and DBE/C should attribute to the non-chromophoric or weak absorptive S-containing compounds. This study supplied an effective evaluation method to compare BrC emissions and their absorption for coal combustion on regional scale.

Selenium is an indispensable trace element for humans and other organisms; however, excessive selenium in water can jeopardize the aquatic environment. Investigations on the biogeochemical cycle of selenium have shown that anthropogenic activities such as mining, refinery, and coal combustion mainly contribute to aquatic selenium pollution, imposing tremendous risks on ecosystems and human beings. Various technologies thus have been developed recently to treat selenium contaminated water to reduce its environmental impacts. This work provides a critical review on the applications, characteristics, and latest developments of current treatment technologies for selenium polluted water. It first outlines the present status of the characteristics, sources, and toxicity of selenium in water. Selenium treatment technologies are then classified into three categories: 1) physicochemical separation including membrane filtration, adsorption, coagulation/precipitation, 2) redox decontamination including chemical reduction and catalysis, and 3) biological transformation including microbial treatment and constructed wetland. Details of these methods including their overall efficiencies, applicability, advantages and drawbacks, and latest developments are systematically analyzed and compared. Although all these methods are promising in treating selenium in water, further studies are still needed to develop sustainable strategies based on existing and new technologies. Perspectives on future research directions are laid out at the end.

Black carbon (BC) aerosol negatively affects air quality and contributes to climate warming globally. However, little is known about the relative contributions of different source control measures to BC reduction owing to the lack of powerful source-diagnostic tools. We combine the fingerprints of dual-carbon isotope using an optimized Bayesian Markov chain Monte Carlo (MCMC) scheme and for the first time to study the key sources of BC in megacity Guangzhou of the Pearl River Delta (PRD) region, China in 2018 autumn season. The MCMC model-derived source apportionment of BC shows that the dominant contributor is petroleum combustion (39%), followed by coal combustion (34%) and biomass burning (27%). It should be noted that the BC source pattern is highly sensitive to the variations of air masses transported with an enhanced contribution of fossil source from the eastern area, suggesting the important impact of regional atmospheric transportation on the BC source profile in the PRD region. Also, we further found that fossil fuel combustion BC contributed 84% to the total BC reduction during 2013–2018. The response of PM₂.₅ concentration to the ¹⁴C-derived BC source apportionment is successfully fitted (r = 0.90) and the results predicted that it would take ∼6 years to reach the WHO PM₂.₅ guideline value (10 μg m⁻³) for the PRD region if the emission control measures keep same as they are at present. Taken together, our findings suggest that dual-carbon isotope is a powerful tool in constraining the source apportionment of BC for the evaluations of air pollution control and carbon emission measures.

Wet deposition is a dominant removal pathway of carbonaceous particles from the atmosphere, but few studies have assessed the particulate carbon in precipitation in Chinese cities. To assess the characteristics and sources of particulate carbon, we measured the concentrations, fluxes, stable carbon isotopes, and radiocarbon of particulate carbon, and some cations concentrations in precipitation in Xi'an, China, in 2019. In contrast to rainfall samples, particulate carbon in snowfall samples in Xi'an showed extremely high concentrations and wet deposition fluxes. The concentrations as well as wet deposition fluxes showed no significant (p > 0.05) differences between urban and suburban sites, and they also exhibited low seasonality in rainfall samples. Water-insoluble organic carbon (WIOC) accounted for the majority (∼90%) of the concentrations and wet deposition fluxes of water-insoluble total carbon (WITC) in precipitation. The best estimates of source apportionment of WITC in precipitation showed that biological sources were the main contributor (80.0% ± 10.5%) in summer, and their contributions decreased to 47.3% ± 12.8% in winter. The contribution of vehicle exhaust emissions accounted for 11.7% ± 3.5% in summer and 39.0% ± 4.3% in winter, while the contributions of coal combustion were relatively small in summer (8.3% ± 7.0%) and winter (13.8% ± 8.5%). Biomass burning accounted for 25.7% ± 9.3% and 89.9% ± 0.7% of the biological sources in summer and winter, respectively, with the remainder comprising other sources of contemporary carbon. These results highlight the nonnegligible contributions of biogenic emissions and biomass burning to particulate carbon in precipitation in this city in summer and winter, respectively.

Inhalation of respirable silica particles can cause serious lung diseases (e.g., silicosis and lung cancer), and the toxicity of respirable silica is highly dependent on its crystal form. Common combustion processes such as coal and biomass burning can provide high temperature environments that may alter the crystal forms of silica and thus affect its toxic effects. Although crystalline silica (i.e., quartz, tridymite, and cristobalite) were widely found at different temperatures during the burning processes, the sources and crystal transformation pathways of silica in the burning processes are still not well understood. Here, we investigate the crystal transformation of silica in the coal and biomass combustion processes and clarify the detailed transformation pathways of silica for the first time. Specifically, in coal burning process, amorphous silica can transform into quartz and cristobalite starting at 1100 °C, and quartz transforms into cristobalite starting at 1200 °C; in biomass burning process, amorphous silica can transform into cristobalite starting at 800 °C, and cristobalite transforms into tridymite starting at 1000 °C. These transformation temperatures are significantly lower than those predicted by the classic theory due to possibly the catalysis of coexisting metal elements (e.g., aluminum, iron, and potassium). Our results not only enable a deeper understanding on the combustion-induced crystal transformation of silica, but also contribute to the mitigation of population exposure to respirable silica.

Heavy metal (loid)s (HMs) and polycyclic aromatic hydrocarbons (PAHs) in soils from a typical industrial county of Shanxi were synchronously measured to determine the spatial clustering of combined HMs and PAHs pollution, and the resulting source-specific health risks. The spatial interaction of HMs and PAHs was determined by the Moran's I index, and a bivariate local indicators of spatial association (LISA) analysis showed that the high HMs-high PAHs clusters were mainly distributed in Fencheng and Xijia towns, as well as the main urban areas of Xiangfen County. The spatial clusters of high naphthalene (Nap)-high HMs were more obvious than those of high benzo(a)pyrene (Bap)-high HMs. Based on positive matrix factorization (PMF), four sources were identified for both HMs and PAHs, with coal consumption and industrial emission identified as common sources of both pollutants. The source-oriented health risk was determined using an improved health risk assessment model. The cancer risk from the combined pollution industrial emissions was relatively serious for both adults and children, with the risk value exceeding 10⁻⁶. Therefore, special attention should be paid to emission control. Based on spatial clustering and source-specific health risk assessment, the largest risk areas and pollutant sources were in the main urban areas of Fencheng and Xijia towns. The spatial interaction patterns and source-specific HMs and PAHs pollution concentrations provide a basis for effective pollution management and control. Finally, a systematic framework for reference was proposed for risk area identification and analysis of the source-oriented health risks of combined HMs and PAHs pollution.

To better promote environment friendly development of the coal chemical industry, this study investigated effects of methanol, sodium citrate, and chlorella powder (a type of microalgae) as co-metabolic substances on enhanced anaerobic treatment of coal pyrolysis wastewater with anaerobic sludge. The anaerobic sludge was loaded into four 2 L anaerobic reactors for co-metabolism enhanced anaerobic experiments. Anaerobic reactor 1 (R1) as control group did not add a co-metabolic substance; anaerobic reactor 2 (R2) added methanol; anaerobic reactor 3 (R3) added sodium citrate; and anaerobic reactor 4 (R4) added chlorella powder. In the blank control group, the removal ratios of total phenol (TPh), quinoline, and indole were only 12.07%, 42.15%, and 50.47%, respectively, indicating that 50 mg/L quinoline, 50 mg/L indole, and 600 mg/L TPh produced strong toxicity inhibition function on the anaerobic microorganism in reactor. When the concentration of methanol, sodium citrate, and chlorella was 400 μg/L, the reactors with co-metabolic substances had better treatment effect on TPh. Among them, the strengthening effects of sodium citrate (TPh removal ratio: 44.87%) and chlorella (47.85%) were better than that of methanol (38.72%) and the control group (10.62%). Additionally, the reactors with co-metabolic substances had higher degradation ratios on quinoline, indole, and chemical oxygen demand (COD). The data of extracellular polymeric substances showed that with the co-metabolic substances, anaerobic microorganisms produced more humic acids by degrading phenols and nitrogen-containing heterocyclic compounds (NHCs). Compared with the control group, the reactors added with sodium citrate and chlorella had larger average particle size of sludge. Thus, sodium citrate and chlorella could improve sludge sedimentation performance by increasing the sludge particle size. The bacterial community structures of reactors were explored and the results showed that Aminicenantes genera incertae sedis, Levinea, Geobacter, Smithella, Brachymonas, and Longilinea were the main functional bacteria in reactor added with chlorella.